%0 Journal Article %T Cu/CuxO/Graphdiyne Tandem Catalyst for Efficient Electrocatalytic Nitrate Reduction to Ammonia. %A Feng X %A Liu J %A Kong Y %A Zhang Z %A Zhang Z %A Li S %A Tong L %A Gao X %A Zhang J %J Adv Mater %V 0 %N 0 %D 2024 Jun 17 %M 38884637 %F 32.086 %R 10.1002/adma.202405660 %X The electrocatalytic reduction reaction of nitrate (NO3 -) to ammonia (NH3) is a feasible way to achieve artificial nitrogen cycle. However, the low yield rate and poor selectivity toward NH3 product is a technical challenge. Here a graphdiyne (GDY)-based tandem catalyst featuring Cu/CuxO nanoparticles anchored to GDY support (termed Cu/CuxO/GDY) for efficient electrocatalytic NO3 - reduction is presented. A high NH3 yield rate of 25.4 mg h-1 mgcat. -1 (25.4 mg h-1 cm-2) with a Faradaic efficiency of 99.8% at an applied potential of -0.8 V versus RHE using the designed catalyst is achieved. These performance metrics outperform most reported NO3 - to NH3 catalysts in the alkaline media. Electrochemical measurements and density functional theory reveal that the NO3 - preferentially attacks Cu/CuxO, and the GDY can effectively catalyze the reduction of NO2 - to NH3. This work highlights the efficacy of GDY as a new class of tandem catalysts for the artificial nitrogen cycle and provides powerful guidelines for the design of tandem electrocatalysts.